We report that multi-junction all-perovskite tandem solar cells are a promising choice for next-generation solar cells with high efficiency and low fabrication cost. However, the lack of high-quality low-bandgap perovskite absorber layers seriously hampers the development of efficient and stable two-terminal monolithic all-perovskite tandem solar cells. Here, we report a bulk-passivation strategy via incorporation of chlorine, to enlarge grains and reduce electronic disorder in mixed tin-lead low-bandgap (~1.25 eV) perovskite absorber layers. This enables the fabrication of efficient low-bandgap perovskite solar cells using thick absorber layers (~750 nm), which is a requisite for efficient tandem solar cells. Such improvement enablesmore » the fabrication of two-terminal all-perovskite tandem solar cells with a champion power conversion efficiency of 21% and steady-state efficiency of 20.7%. Finally, the efficiency is retained to 85% of its initial performance after 80 h of operation under continuous illumination.« less

We report the unsatisfactory performance of low-bandgap mixed tin (Sn)-lead (Pb) halide perovskite subcells has been one of the major obstacles hindering the progress of the power conversion efficiencies (PCEs) of all-perovskite tandem solar cells. By analyzing dark-current density and distribution, it is identified that charge recombination at grain boundaries is a key factor limiting the performance of low-bandgap mixed Sn-Pb halide perovskite subcells. It is further found that bromine (Br) incorporation can effectively passivate grain boundaries and lower the dark current density by two-three orders of magnitude. By optimizing the Br concentration, low-bandgap (1.272 eV) mixed Sn-Pb halide perovskitemore » solar cells are fabricated with open-circuit voltage deficits as low as 0.384 V and fill factors as high as 75%. The best-performing device demonstrates a PCE of >19%. In conclusion, the results suggest an important direction for improving the performance of low-bandgap mixed Sn-Pb halide perovskite solar cells.« less

Multijunction solar cells based on epitaxially grown III-V materials hold the record for solar energy power conversion efficiency (PCE). However, due to the high cost of fabricating these devices, they are typically only used for concentrator cells and space applications. The overarching goal of this project was to develop low-cost printable hybrid perovskite (HP) materials appropriate and optimized for tandem solar cells with high power conversion efficiency under “1 Sun” illumination. Key results and findings over the course of the project we: Developed higher-performance high-bandgap (1.75 eV) perovskite materials and devices. In particular, we explored tens-of-thousands of compositions for highmore » bandgap perovskites, achieving quasi-Fermi level splitting of 1.35 eV for a 1.75 eV bandgap material. We achieved World-record open circuit voltages from single junction p-i-n devices, 1.24 V from 1.75 eV bandgap material, which is what is preferable for tandems with a PCE of 14.3% using a guanidinium/formanadinium/ cesium alloyed lead iodobromide. We also developed a series of World-record efficiency devices at higher band-gaps based on 2D/3D perovskites using PEA. Developed higher-performance low-bandgap (1.35 eV) perovskite materials and devices. In particular, we developed a 1.35 eV bandgap perovskite of composition MAPb0.5Sn0.5(I0.8Br0.2)3 and showed its superiority to MAPb0.75Sn0.25I3. High efficiency solar cells were fabricated using PEDOT:PSS and doped-ICBA as HTL and ETL, respectively. Short circuit currents of 25.7 mA/cm2 and PCEs of 17.1% were obtained. Developed mechanically stacked 4-terminal CIGS-Perovskite tandems with PCE of 18.8% and monolithic 2-terminal CIGS-Perovskite tandems with PCE of 8.5%. The low efficiency of the monolithic device is a result of the high surface roughness of the solution processed CIGS bottom cells. This is not an intrinsic problem for CIGS-perovskite tandems, but does mean that smooth evaporated or sputtered CIGS films likely need to be used, unless a polishing step is employed. Developed monolithic 2-terminal Perovskite-Perovskite tandems with a stabilized PCE of 18.5%. This was the World-record perovskite-perovskite monolithic tandems for over a year in 2017-2018. Revealed that light is not an essential component of the so-called “light-induced” phase segregation. By using charge injection in the dark and electroluminescence, we showed that the presence of electrons in the conduction band and hole in the valence band is sufficient to drive the nearly ubiquitously observed phase segregation in high bandgap perovskites. Developed a new method to simultaneously measure absolute intensity photoluminescence and photoconductivity and use them to obtain simultaneous in-situ measurement of quasi-Fermi level splitting and diffusion length. This is important since it provides a proxy for device Voc and device Jsc. In addition, 67 papers were published with support from this award that detail many more advances in the field, including numerous publications in high impact journals such as Nature Photonics, Advanced Materials, ACS Energy Letters, and Energy and Environmental Science.« less

All-perovskite–based polycrystalline thin-film tandem solar cells have the potential to deliver efficiencies of >30%. However, the performance of all-perovskite–based tandem devices has been limited by the lack of high-efficiency, low–band gap tin-lead (Sn-Pb) mixed-perovskite solar cells (PSCs). We found that the addition of guanidinium thiocyanate (GuaSCN) resulted in marked improvements in the structural and optoelectronic properties of Sn-Pb mixed, low–band gap (~1.25 electron volt) perovskite films. The films have defect densities that are lower by a factor of 10, leading to carrier lifetimes of greater than 1 microsecond and diffusion lengths of 2.5 micrometers. These improved properties enable our demonstrationmore » of >20% efficient low–band gap PSCs. When combined with wider–band gap PSCs, we achieve 25% efficient four-terminal and 23.1% efficient two-terminal all-perovskite–based polycrystalline thin-film tandem solar cells.« less

Wide-bandgap perovskites are attractive top-cell materials for tandem photovoltaic applications. Comprehensive optical modeling is essential to minimize the optical losses of state-of-the-art perovskite/perovskite, perovskite/CIGS, and perovskite/silicon tandems. Such models require accurate optical constants of wide-bandgap perovskites. Here, we report optical constants determined with ellipsometry and spectrophotometry for two new wide-bandgap, cesium-formamidinium-based perovskites. We validate the optical constants by comparing simulated quantum efficiency and reflectance spectra with measured cell results for semi-transparent single-junction perovskite cells and find less than 0.3 mA/cm 2 error in the short-circuit current densities. Such simulations further reveal that reflection and parasitic absorption in the front ITOmore » layer and electron contact are responsible for the biggest optical losses. We also show that the complex refractive index of methylammonium lead triiodide, the most common perovskite absorber for solar cells, can be used to generate approximate optical constants for an arbitrary wide-bandgap perovskite by translating the data along the wavelength axis. Finally, these optical constants are used to map the short-circuit current density of a textured two-terminal perovskite/silicon tandem solar cell as a function of the perovskite thickness and bandgap, providing a guide to nearly 20 mA/cm 2 matched current density with any perovskite bandgap between 1.56 and 1.68 eV.« less